EP0554721A1 - Procédé de préparation de mousses souples, élastiques de PUR à cellules ouvertes - Google Patents

Procédé de préparation de mousses souples, élastiques de PUR à cellules ouvertes Download PDF

Info

Publication number
EP0554721A1
EP0554721A1 EP93100877A EP93100877A EP0554721A1 EP 0554721 A1 EP0554721 A1 EP 0554721A1 EP 93100877 A EP93100877 A EP 93100877A EP 93100877 A EP93100877 A EP 93100877A EP 0554721 A1 EP0554721 A1 EP 0554721A1
Authority
EP
European Patent Office
Prior art keywords
weight
molecular weight
bis
optionally
known per
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP93100877A
Other languages
German (de)
English (en)
Other versions
EP0554721B1 (fr
Inventor
Sven Dr. Meyer-Ahrens
Gundolf Dr. Jacobs
Hans Dr. Hettel
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Bayer AG
Original Assignee
Bayer AG
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Bayer AG filed Critical Bayer AG
Publication of EP0554721A1 publication Critical patent/EP0554721A1/fr
Application granted granted Critical
Publication of EP0554721B1 publication Critical patent/EP0554721B1/fr
Anticipated expiration legal-status Critical
Expired - Lifetime legal-status Critical Current

Links

Classifications

    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G18/00Polymeric products of isocyanates or isothiocyanates
    • C08G18/06Polymeric products of isocyanates or isothiocyanates with compounds having active hydrogen
    • C08G18/28Polymeric products of isocyanates or isothiocyanates with compounds having active hydrogen characterised by the compounds used containing active hydrogen
    • C08G18/40High-molecular-weight compounds
    • C08G18/48Polyethers
    • C08G18/4804Two or more polyethers of different physical or chemical nature
    • C08G18/4812Mixtures of polyetherdiols with polyetherpolyols having at least three hydroxy groups
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G18/00Polymeric products of isocyanates or isothiocyanates
    • C08G18/06Polymeric products of isocyanates or isothiocyanates with compounds having active hydrogen
    • C08G18/28Polymeric products of isocyanates or isothiocyanates with compounds having active hydrogen characterised by the compounds used containing active hydrogen
    • C08G18/40High-molecular-weight compounds
    • C08G18/48Polyethers
    • C08G18/4804Two or more polyethers of different physical or chemical nature
    • C08G18/4816Two or more polyethers of different physical or chemical nature mixtures of two or more polyetherpolyols having at least three hydroxy groups
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2110/00Foam properties
    • C08G2110/0008Foam properties flexible
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2110/00Foam properties
    • C08G2110/0041Foam properties having specified density
    • C08G2110/005< 50kg/m3
    • CCHEMISTRY; METALLURGY
    • C08ORGANIC MACROMOLECULAR COMPOUNDS; THEIR PREPARATION OR CHEMICAL WORKING-UP; COMPOSITIONS BASED THEREON
    • C08GMACROMOLECULAR COMPOUNDS OBTAINED OTHERWISE THAN BY REACTIONS ONLY INVOLVING UNSATURATED CARBON-TO-CARBON BONDS
    • C08G2110/00Foam properties
    • C08G2110/0083Foam properties prepared using water as the sole blowing agent

Definitions

  • PUR flexible foams are used in a variety of ways as upholstery materials in the furniture and vehicle sectors.
  • physical blowing agents such as Monofluorotrichloromethane (R11) use because, unlike water, they do not increase the polyurea content of the polymer.
  • the object of the present invention is therefore to adjust the compression hardness of PUR flexible foams (hot foams) in the desired manner without using the physical blowing agents used hitherto.
  • open-celled PUR block foams can be produced with reduced hardness and good elasticity if small amounts of oxyethylene group-rich polyethers (oxyethylene group content> 50%, functionality at least two) are used and at the same time in the range of 95 (index range) between 95 and 110 works.
  • oxyethylene group-rich polyethers oxyethylene group content> 50%, functionality at least two
  • the process thus enables the compression hardness to be reduced by more than 40% with an excellent value level, especially with high foam elasticity
  • Surface-active additives such as emulsifiers and foam stabilizers, also cell regulators of the type known per se, such as paraffins or fatty alcohols or dimethylpolysiloxanes, and pigments or dyes and flame retardants of the type known per se, for example trischloroethyl phosphate, triscresyl phosphate, further stabilizers against aging and weather influences, plasticizers and fungistatic Bacteriostatic substances as well as fillers such as barium sulfate, diatomaceous earth, soot or chalk.
  • emulsifiers and foam stabilizers also cell regulators of the type known per se, such as paraffins or fatty alcohols or dimethylpolysiloxanes, and pigments or dyes and flame retardants of the type known per se, for example trischloroethyl phosphate, triscresyl phosphate, further stabilizers against aging and weather influences, plasticizers and fungistatic Bacteriostatic substances as well as
  • surface-active additives and foam stabilizers to be used according to the invention, as well as cell regulators, reaction retarders, stabilizers, flame-retardant substances, plasticizers, dyes and fillers, as well as fungistatic and bacteriostatic substances and Details on the use and mode of action of these additives are described in the Plastics Manual, Volume VII, edited by Vieweg and Höchtlen, Carl-Hanser-Verlag, Kunststoff 1966, eg on pages 103 to 113.
  • the reaction components are reacted according to the one-step process, the prepolymer process or the semi-prepolymer process, which are known per se, machine equipment often being used, e.g. those described in U.S. Patent No. 2,764,565. Details on processing devices that are also suitable according to the invention are given in the plastics manual, volume VII, published by Vieweg and Höchtlen, Carl-Hanser-Verlag, Kunststoff 1966, e.g. on pages 121 to 205.
  • all components are implemented with a characteristic number (isocyanate index) of 95 to 110, preferably with a characteristic number of 9 8 to 100.
  • the key figure a term used very often in the production of polyurethane foams, says something about the degree of crosslinking of a foam. It is customary to consider that foam with the code number 100 that has the stoichiometric ratio or the theoretically required amount of isocyanate was used. With the help of the key figure it is possible to define the degree of under- or over-networking in more detail.
  • the key figure is calculated according to the general formula as follows:
  • the flexible polyurethane foams obtainable according to the invention are used, for example, as reclining and seating furniture, seats in means of transport, preferably in the car.
  • Polyol B PO / EO adduct of glycerol with an oxyethylene group content of approx. 72% by weight, predominantly prim. OH groups and an average molecular weight of about 4,700.
EP93100877A 1992-02-03 1993-01-21 Procédé de préparation de mousses souples, élastiques de PUR à cellules ouvertes Expired - Lifetime EP0554721B1 (fr)

Applications Claiming Priority (2)

Application Number Priority Date Filing Date Title
DE4202992 1992-02-03
DE4202992A DE4202992A1 (de) 1992-02-03 1992-02-03 Verfahren zur herstellung von elastischen, offenzelligen pur-weichschaumstoffen

Publications (2)

Publication Number Publication Date
EP0554721A1 true EP0554721A1 (fr) 1993-08-11
EP0554721B1 EP0554721B1 (fr) 1997-10-29

Family

ID=6450843

Family Applications (1)

Application Number Title Priority Date Filing Date
EP93100877A Expired - Lifetime EP0554721B1 (fr) 1992-02-03 1993-01-21 Procédé de préparation de mousses souples, élastiques de PUR à cellules ouvertes

Country Status (8)

Country Link
EP (1) EP0554721B1 (fr)
JP (1) JPH05271379A (fr)
AT (1) ATE159740T1 (fr)
CA (1) CA2088414C (fr)
DE (2) DE4202992A1 (fr)
DK (1) DK0554721T3 (fr)
ES (1) ES2108142T3 (fr)
NO (1) NO302891B1 (fr)

Cited By (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0845485A1 (fr) * 1996-12-02 1998-06-03 Bayer Ag Mousses de polyuréthane souples et élastiques et leur procédé de préparation
US6774153B2 (en) 2000-01-17 2004-08-10 Huntsman International Llc Process for preparing a free rise or slabstock flexible polyurethane foam
US6919384B2 (en) 2001-02-26 2005-07-19 Huntsman International Llc Process for preparing a flexible polyurethane foam
ITMI20092227A1 (it) * 2009-12-18 2011-06-19 Dow Global Technologies Inc Schiume poliuretaniche ritardanti di fiamma contenenti legami biureto

Families Citing this family (3)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE19924802B4 (de) * 1999-05-29 2008-02-28 Basf Ag Verfahren zur Herstellung von schalldämpfenden und energieabsorbierenden Polyurethanschäumen
MXPA02007859A (es) 2000-02-14 2002-11-29 Huntsman Int Llc Proceso para preparar una espuma flexible de poliuretano.
JP5839394B2 (ja) * 2011-11-02 2016-01-06 株式会社イノアックコーポレーション 寝具用クッション

Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2211914A1 (de) * 1971-03-15 1972-10-12 Pechiney Ugine Kuhlmann Herstellung von Polyurethan-Schaumstoffen mit sehr geringer Stauchhärte und hohem Aufsaugvermögen
GB1480972A (en) * 1974-04-19 1977-07-27 Naphtachimie Sa Process for manufacturing polyurethane foams having elasticity
EP0116309A1 (fr) * 1983-01-17 1984-08-22 Basf Wyandotte Corporation Mousses de polyuréthane flexibles ayant une déformation sous charge à pression de bille préparées à partir de mélanges de polyols
EP0433889A2 (fr) * 1989-12-21 1991-06-26 BASF Aktiengesellschaft Procédé de préparation de mousses souples de polyuréthane à faible résistance à la compression et mélanges de polyols séquencés de polyoxypropylène-polyoxyéthylène adaptés à ce procédé

Patent Citations (4)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
DE2211914A1 (de) * 1971-03-15 1972-10-12 Pechiney Ugine Kuhlmann Herstellung von Polyurethan-Schaumstoffen mit sehr geringer Stauchhärte und hohem Aufsaugvermögen
GB1480972A (en) * 1974-04-19 1977-07-27 Naphtachimie Sa Process for manufacturing polyurethane foams having elasticity
EP0116309A1 (fr) * 1983-01-17 1984-08-22 Basf Wyandotte Corporation Mousses de polyuréthane flexibles ayant une déformation sous charge à pression de bille préparées à partir de mélanges de polyols
EP0433889A2 (fr) * 1989-12-21 1991-06-26 BASF Aktiengesellschaft Procédé de préparation de mousses souples de polyuréthane à faible résistance à la compression et mélanges de polyols séquencés de polyoxypropylène-polyoxyéthylène adaptés à ce procédé

Cited By (5)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
EP0845485A1 (fr) * 1996-12-02 1998-06-03 Bayer Ag Mousses de polyuréthane souples et élastiques et leur procédé de préparation
US6774153B2 (en) 2000-01-17 2004-08-10 Huntsman International Llc Process for preparing a free rise or slabstock flexible polyurethane foam
US6919384B2 (en) 2001-02-26 2005-07-19 Huntsman International Llc Process for preparing a flexible polyurethane foam
ITMI20092227A1 (it) * 2009-12-18 2011-06-19 Dow Global Technologies Inc Schiume poliuretaniche ritardanti di fiamma contenenti legami biureto
WO2011073355A1 (fr) * 2009-12-18 2011-06-23 Dow Global Technologies Inc. Mousses de polyuréthane ignifuges contenant des liaisons biurets

Also Published As

Publication number Publication date
NO930181L (no) 1993-08-04
CA2088414C (fr) 2004-07-06
DK0554721T3 (da) 1998-07-20
ES2108142T3 (es) 1997-12-16
NO302891B1 (no) 1998-05-04
DE59307585D1 (de) 1997-12-04
EP0554721B1 (fr) 1997-10-29
ATE159740T1 (de) 1997-11-15
JPH05271379A (ja) 1993-10-19
DE4202992A1 (de) 1993-08-05
CA2088414A1 (fr) 1993-08-04
NO930181D0 (no) 1993-01-19

Similar Documents

Publication Publication Date Title
EP0344551B1 (fr) Mélanges de polyisocyanates liquides un procédé pour leur préparation et leur utilisation pour la préparation de mousses de polyuréthane souples
EP0331941B1 (fr) Procédé de préparation de mousses de polyuréthane flexibles, durcissant à froid et ayant d&#39;excellentes propriétés d&#39;assourdissement
EP1797129B1 (fr) Procede pour produire des mousses souples de polyurethane
EP1756187B1 (fr) Mousses polyurethane de faible densite et leur utilisation dans des semelles de chaussures
EP1650240B1 (fr) Mousse flexible de polyurethane ayant une faible densité et à résistance réduite à la compression
EP0555721A1 (fr) Procédé de préparation de mousses de polyuréthane flexibles durcissant à froid
EP0346670B1 (fr) Procédé de préparation de mousses souples de polyuréthane
DE3721058A1 (de) Verfahren zur herstellung von kalthaertenden polyurethan-weichformschaumstoffen
EP0439792B1 (fr) Mélanges de polyisocyanates et leur utilisation pour la préparation de mousses de polyuréthane flexibles
EP0499053B1 (fr) Procédé de préparation d&#39;élastomères de polyuréthane et compositions de polyoxybutylène-polyoxyalcoylène-glycols et de composés glycidiliques appropriées à ce procédé
EP1266918A2 (fr) Procédé de fabrication de mousses polyurethanes à grande élasticité
EP0177766B1 (fr) Utilisation de diamines aromatiques stériquement encombrées pour la préparation de mousses de polyuréthanes
EP0463493B1 (fr) Procédé de préparation de mousses rigides contenant des groupes d&#39;uréthane et essentiellement d&#39;isocyanurate et leur utilisation comme matériau isolant
EP1097953A2 (fr) Procédé pour la préparation de mousses de polyuréthane
EP0472080B1 (fr) Procédé de préparation de mousses rigides de polyuréthane
EP0554721B1 (fr) Procédé de préparation de mousses souples, élastiques de PUR à cellules ouvertes
EP0445411B1 (fr) Procédé de préparation de mousses dures à cellules essentiellement fermées ayant des groupes uréthanne, uré et/ou biuret et leur utilisation
DE2509478A1 (de) Verfahren zur herstellung von polyaetherurethanschaeumen mit hoher rueckprallelastizitaet
DE3910100C1 (fr)
EP0693526A1 (fr) Procédé pour la préparation de mousses rigides d&#39;uréthane contenant éventuellement des groupes isocyanurates
EP0373456A2 (fr) Procédé pour la préparation de mousses de polyuréthane hydrophyliques à pores ouverts
EP0445405A2 (fr) Procédé pour préparer des mousses de polyuréthane souples à cellules ouvertes
EP0446468A1 (fr) Mélanges de prépolymères contenant des groupes uréthane avec des diisocyanate-toluènes et leur utilisation
EP0472896B1 (fr) Procédé pour la préparation de mousses flexibles hautement élastiques et leur utilisation comme matériau de rembourrage
EP0563682A1 (fr) Procédé de préparation de mousses souples de polyuréthane durcissables à froid

Legal Events

Date Code Title Description
PUAI Public reference made under article 153(3) epc to a published international application that has entered the european phase

Free format text: ORIGINAL CODE: 0009012

AK Designated contracting states

Kind code of ref document: A1

Designated state(s): AT BE CH DE DK ES FR GB IT LI NL PT SE

17P Request for examination filed

Effective date: 19930901

17Q First examination report despatched

Effective date: 19950912

GRAG Despatch of communication of intention to grant

Free format text: ORIGINAL CODE: EPIDOS AGRA

GRAH Despatch of communication of intention to grant a patent

Free format text: ORIGINAL CODE: EPIDOS IGRA

GRAH Despatch of communication of intention to grant a patent

Free format text: ORIGINAL CODE: EPIDOS IGRA

GRAA (expected) grant

Free format text: ORIGINAL CODE: 0009210

AK Designated contracting states

Kind code of ref document: B1

Designated state(s): AT BE CH DE DK ES FR GB IT LI NL PT SE

REF Corresponds to:

Ref document number: 159740

Country of ref document: AT

Date of ref document: 19971115

Kind code of ref document: T

REG Reference to a national code

Ref country code: CH

Ref legal event code: EP

REG Reference to a national code

Ref country code: CH

Ref legal event code: NV

Representative=s name: E. BLUM & CO. PATENTANWAELTE

REF Corresponds to:

Ref document number: 59307585

Country of ref document: DE

Date of ref document: 19971204

ITF It: translation for a ep patent filed

Owner name: ING. C. GREGORJ S.P.A.

REG Reference to a national code

Ref country code: ES

Ref legal event code: FG2A

Ref document number: 2108142

Country of ref document: ES

Kind code of ref document: T3

GBT Gb: translation of ep patent filed (gb section 77(6)(a)/1977)

Effective date: 19971212

ET Fr: translation filed
REG Reference to a national code

Ref country code: PT

Ref legal event code: SC4A

Free format text: AVAILABILITY OF NATIONAL TRANSLATION

Effective date: 19980108

REG Reference to a national code

Ref country code: DK

Ref legal event code: T3

PLBE No opposition filed within time limit

Free format text: ORIGINAL CODE: 0009261

STAA Information on the status of an ep patent application or granted ep patent

Free format text: STATUS: NO OPPOSITION FILED WITHIN TIME LIMIT

26N No opposition filed
REG Reference to a national code

Ref country code: GB

Ref legal event code: IF02

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: IT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20050121

REG Reference to a national code

Ref country code: CH

Ref legal event code: PFA

Owner name: BAYER AG

Free format text: BAYER AG# #51368 LEVERKUSEN (DE) -TRANSFER TO- BAYER AG# #51368 LEVERKUSEN (DE)

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: DK

Payment date: 20090113

Year of fee payment: 17

Ref country code: AT

Payment date: 20090113

Year of fee payment: 17

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: PT

Payment date: 20090119

Year of fee payment: 17

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: CH

Payment date: 20090114

Year of fee payment: 17

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: SE

Payment date: 20090108

Year of fee payment: 17

PGRI Patent reinstated in contracting state [announced from national office to epo]

Ref country code: IT

Effective date: 20091201

REG Reference to a national code

Ref country code: PT

Ref legal event code: MM4A

Free format text: LAPSE DUE TO NON-PAYMENT OF FEES

Effective date: 20100721

REG Reference to a national code

Ref country code: CH

Ref legal event code: PL

REG Reference to a national code

Ref country code: DK

Ref legal event code: EBP

EUG Se: european patent has lapsed
PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: LI

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20100131

Ref country code: CH

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20100131

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: AT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20100121

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: PT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20100721

Ref country code: DK

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20100131

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: FR

Payment date: 20110128

Year of fee payment: 19

Ref country code: IT

Payment date: 20110119

Year of fee payment: 19

Ref country code: NL

Payment date: 20110117

Year of fee payment: 19

Ref country code: DE

Payment date: 20110104

Year of fee payment: 19

PGFP Annual fee paid to national office [announced via postgrant information from national office to epo]

Ref country code: ES

Payment date: 20110216

Year of fee payment: 19

Ref country code: BE

Payment date: 20110225

Year of fee payment: 19

Ref country code: GB

Payment date: 20110119

Year of fee payment: 19

BERE Be: lapsed

Owner name: *BAYER A.G.

Effective date: 20120131

REG Reference to a national code

Ref country code: NL

Ref legal event code: V1

Effective date: 20120801

GBPC Gb: european patent ceased through non-payment of renewal fee

Effective date: 20120121

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: SE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20100122

REG Reference to a national code

Ref country code: FR

Ref legal event code: ST

Effective date: 20120928

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: GB

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120121

Ref country code: DE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120801

REG Reference to a national code

Ref country code: DE

Ref legal event code: R119

Ref document number: 59307585

Country of ref document: DE

Effective date: 20120801

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: IT

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120121

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: BE

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120131

Ref country code: FR

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120131

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: NL

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120801

REG Reference to a national code

Ref country code: ES

Ref legal event code: FD2A

Effective date: 20130708

PG25 Lapsed in a contracting state [announced via postgrant information from national office to epo]

Ref country code: ES

Free format text: LAPSE BECAUSE OF NON-PAYMENT OF DUE FEES

Effective date: 20120122